EP0091277B1 - Dimethylacetamide solvate of syn-(2-amino thiazol-4-yl)(methoxyimino)acetic acid - Google Patents

Dimethylacetamide solvate of syn-(2-amino thiazol-4-yl)(methoxyimino)acetic acid Download PDF

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Publication number
EP0091277B1
EP0091277B1 EP83301807A EP83301807A EP0091277B1 EP 0091277 B1 EP0091277 B1 EP 0091277B1 EP 83301807 A EP83301807 A EP 83301807A EP 83301807 A EP83301807 A EP 83301807A EP 0091277 B1 EP0091277 B1 EP 0091277B1
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EP
European Patent Office
Prior art keywords
solvate
acetic acid
syn
dimethylacetamide
acid
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired
Application number
EP83301807A
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German (de)
English (en)
French (fr)
Other versions
EP0091277A2 (en
EP0091277A3 (en
Inventor
Robert William Burchfield
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Eli Lilly and Co
Original Assignee
Eli Lilly and Co
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Filing date
Publication date
Application filed by Eli Lilly and Co filed Critical Eli Lilly and Co
Publication of EP0091277A2 publication Critical patent/EP0091277A2/en
Publication of EP0091277A3 publication Critical patent/EP0091277A3/en
Application granted granted Critical
Publication of EP0091277B1 publication Critical patent/EP0091277B1/en
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Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D277/00Heterocyclic compounds containing 1,3-thiazole or hydrogenated 1,3-thiazole rings
    • C07D277/02Heterocyclic compounds containing 1,3-thiazole or hydrogenated 1,3-thiazole rings not condensed with other rings
    • C07D277/20Heterocyclic compounds containing 1,3-thiazole or hydrogenated 1,3-thiazole rings not condensed with other rings having two or three double bonds between ring members or between ring members and non-ring members
    • C07D277/587Heterocyclic compounds containing 1,3-thiazole or hydrogenated 1,3-thiazole rings not condensed with other rings having two or three double bonds between ring members or between ring members and non-ring members with aliphatic hydrocarbon radicals substituted by carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals, directly attached to ring carbon atoms, said aliphatic radicals being substituted in the alpha-position to the ring by a hetero atom, e.g. with m >= 0, Z being a singly or a doubly bound hetero atom
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D275/00Heterocyclic compounds containing 1,2-thiazole or hydrogenated 1,2-thiazole rings
    • C07D275/02Heterocyclic compounds containing 1,2-thiazole or hydrogenated 1,2-thiazole rings not condensed with other rings

Definitions

  • This invention concerns synthetic pharmaceutical chemistry. It provides a new solvate and makes available a new process for purifying syn-(2-aminothiazol-4-yl)(methoxyimino)acetic acid using the solvate.
  • Syn-(2-aminothiazol-4-yl)(methoxyimino)acetic acid is a known compound. It is used as an intermediate in preparing cephalosporin pharmaceuticals of the type having an acyl side chain formed from the thiazolyl acetic acid. Numerous patents and publications disclosing this use have appeared. For example, U.S. Patent 4,152,433 of Fujisawa Co. and U.S. Patent 4,098,888 of Takeda Chemical Industries show the synthesis of various cephalosporin compounds making use of the thiazolylacetic acid as an intermediate. Often the amino group of the substituted acetic acid is blocked by a group such as trityl or the like, and the acid is usually converted into an active form such as the acid chloride or the like for use as an acylating agent.
  • solvates are known to be a highly individualistic effect. The ability of a given compound to form a solvate is not predictable, so far as applicant knows, and to his knowledge and belief nothing in the literature indicates that syn-(2-aminothiazol-4-yl)(methoxyimino)acetic acid can form a solvate with dimethylacetamide, or with any solvent.
  • this invention provides a dimethylacetamide solvate of syn-(2-aminothiazol-4-yl)-(methoxyimino)acetic acid containing 2 moles of dimethylacetamide per mole of the acid.
  • the thiazolyl acetic acid whose solvate is provided by this invention is of the formula It is important that the methoxyimino group be in the configuration shown, known as the syn configuration, because it is now well known that the cephalosporins formed from the acid are much more biologically active when the imino group is in the syn configuration.
  • the dimethylacetamide (DMAC) disolvate of the acid is readily formed by merely dissolving the impure solid acid in DMAC, and crystallizing the solvate from the solution.
  • the crystallization may be done by the usual methods, such as cooling or chilling a solution made at an elevated temperature, or evaporating part of the DMAC from the solution.
  • the formation of the DMAC disolvate is a simple crystallization from DMAC.
  • the formation and precipitation of the disolvate are analogous to other crystallization procedures.
  • the yield of disolvate is increased by higher concentration of the acid and by lower crystallization temperature, and decreased by lower concentration and higher crystallization temperature.
  • the composition and purity of the precipitated disolvate are not affected by the conditions, however. Accordingly, the chemist can vary the amount of DMAC and the temperatures freely. For example, concentrations of the acid in the range of from about 5% to about 50% by weight may be used as may be desired in a given case.
  • the DMAC solution of the acid may be heated, to obtain dissolution, to temperatures in the range of from about the ambient temperature to about 100°C, or even higher, using elevated pressures as necessary to suppress boiling.
  • the solution may be cooled, to obtain crystallization, to any temperature short of that which completely solidifies the solution, such as from about -50°C to about the ambient temperature.
  • a process for preparing a dimethylacetamide solvate of syn-(2-aminothiazol-4-yl)(methoxyimino)acetic acid the solvate containing 2 moles of dimethylacetamide per mole of acid, which comprises dissolving impure syn-(2-aminothiazol-4-yl)-(methoxyimino)acetic acid in dimethylacetamide and crystallizing the solvate.
  • the precipitated disolvate is easily removed from the liquid phase by filtration or centrifugation, and can be washed on the filter with DMAC or other solvents to remove liquid phase containing the impurities which have been removed from the acid.
  • the solvate of this invention is a true solvate having a fixed composition, but it is not tightly bound.
  • the DMAC is easily removed from the solvate with heat and vacuum, if the dry pure acid is needed for use as an intermediate.
  • the solvent for the next synthetic step is DMAC, or if a small amount of DMAC is acceptable in the reaction mixture, the solvate may be used as the intermediate without further treatment.
  • the DMAC is readily removed from the solvate of this invention by simple contact with water, or with virtually any convenient organic solvent. It is unnecessary to dissolve the solvate to remove the DMAC. As the examples below illustrate, mere slurrying of the solvate in an organic solvent or water will remove the DMAC into the solvent phase, so that the acid may be obtained in pure form by filtering.
  • ethers such as diethyl ether, tetrahydrofuran and diisopropyl ether, alcohols such as methanol, ethanol and butanol, alkanes such as hexane, octane and the like, haloalkanes such as dichloromethane, 1,2-dichloroethane and trichloroethane, aromatics and halo-aromatics such as benzene, toluene, xylene, chlorobenzene, bromobenzene and the dichlorobenzenes, amides such as dimethylformamide, and ketones such as acetone, methyl ethyl ketone and methyl isobutyl ketone may be used.
  • a process for purifying syn-(2-aminothiazol-4-yl)(methoxyimino)acetic acid comprising dissolving impure syn-(2-aminothiazol-4-yl)-(methoximino)acetic acid in dimethylacetamide, crystallizing the dimethylacetamide solvate, removing the solvate from the solution, and removing the dimethylacetamide from the solvate.
  • the method of purification is especially useful for purifying water-wet acid. It is found that water is particularly difficult to remove from the acid, and normal drying techniques are inadequate.
  • the purification method of this invention precipitates the disolvate quite free of water, even when the impure acid contains several percent of water, and accordingly produces the acid in a form which is much more appropriate for further processing.
  • the present method also is particularly efficient in purifying the acid from the dark, tarry contaminants which usually are formed in its synthesis.
  • the solvate precipitates as cubic white crystals, leaving the dark matter in the DMAC phase. It will be understood that dark-colored impurities are very undesirable in intermediates to be used for synthesis, especially in pharmaceutical intermediates.
  • the solvate may be used as an intermediate, just as it is precipitated, if a small amount of DMAC is . acceptable in the reaction mixture in which it is to serve as an intermediate. If DMAC is not acceptable, the DMAC can be removed by drying, or displaced with water, if the next reaction mixture is aqueous, or with any convenient organic solvent, if water is not acceptable in that next reaction mixture.
  • the disolvate was suspended in 400 ml of ethyl acetate and stirred for 2 hours at 45°C under nitrogen. The suspension was then cooled to 10°C and filtered, and the solids were washed with 800 ml of additional ethyl acetate. The washed solids were dried for two and a half hours in air at 50°C, and 44.4 g of dried product was obtained, which was identified as 97.26% pure syn-(2-aminothiazol-4-yl)(methoximino)acetic acid containing 1.35% of DMAC and 1.37% of ethyl acetate. The water content of the product was 0.36% by Karl Fischer analysis. M.P. 130-131 0 C.
  • the solid disolvate was washed with 200 ml of 1:4 DMAC:ethyl acetate, 200 ml of 1:19 DMAC:ethyl acetate and finally with 400 ml of ethyl acetate.
  • the solid disolvate was perfectly white and the cake was crystalline and easily handled. M.P. 60-66°C.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Cephalosporin Compounds (AREA)
  • Thiazole And Isothizaole Compounds (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
EP83301807A 1982-04-01 1983-03-30 Dimethylacetamide solvate of syn-(2-amino thiazol-4-yl)(methoxyimino)acetic acid Expired EP0091277B1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US06/364,356 US4426528A (en) 1982-04-01 1982-04-01 Purification of syn-(2-aminothiazol-4-yl)methoxyimino)acetic acid
US364356 1982-04-01

Publications (3)

Publication Number Publication Date
EP0091277A2 EP0091277A2 (en) 1983-10-12
EP0091277A3 EP0091277A3 (en) 1984-12-27
EP0091277B1 true EP0091277B1 (en) 1987-06-16

Family

ID=23434150

Family Applications (1)

Application Number Title Priority Date Filing Date
EP83301807A Expired EP0091277B1 (en) 1982-04-01 1983-03-30 Dimethylacetamide solvate of syn-(2-amino thiazol-4-yl)(methoxyimino)acetic acid

Country Status (11)

Country Link
US (1) US4426528A (OSRAM)
EP (1) EP0091277B1 (OSRAM)
JP (1) JPS58183678A (OSRAM)
KR (1) KR840004090A (OSRAM)
CA (1) CA1194487A (OSRAM)
DE (1) DE3372096D1 (OSRAM)
DK (1) DK91383A (OSRAM)
GB (1) GB2119370B (OSRAM)
GR (1) GR79243B (OSRAM)
HU (1) HU186271B (OSRAM)
IL (1) IL68251A (OSRAM)

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS6124580A (ja) * 1984-07-12 1986-02-03 Shionogi & Co Ltd アミノチアゾリルグルタル酸誘導体の製造方法
AU2002222553A1 (en) * 2000-12-04 2002-06-18 Fujisawa Pharmaceutical Co. Ltd. Process for producing anhydride of aminothiazole derivative
CN111548323B (zh) * 2020-05-29 2022-06-10 山东金城医药化工有限公司 氨噻肟酸的回收方法

Family Cites Families (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3925372A (en) 1973-02-23 1975-12-09 Lilly Co Eli Alpha-aminoacyl-3-halo cephalosporins
DK154939C (da) 1974-12-19 1989-06-12 Takeda Chemical Industries Ltd Analogifremgangsmaade til fremstilling af thiazolylacetamido-cephemforbindelser eller farmaceutisk acceptable salte eller estere deraf
DE2760123C2 (de) 1976-01-23 1986-04-30 Roussel-Uclaf, Paris 7-Aminothiazolyl-syn-oxyiminoacetamidocephalosporansäuren, ihre Herstellung und sie enthaltende pharmazeutische Zusammensetzungen
US4152433A (en) 1976-03-12 1979-05-01 Fujisawa Pharmaceutical Co., Ltd. 2-Lower alkyl-7-substituted-2 or 3-cephem-4-carboxylic acid compounds and pharmaceutical compositions
DK162391C (da) * 1976-04-12 1992-03-09 Fujisawa Pharmaceutical Co Analogifremgangsmaade til fremstilling af syn-isomerer af 3,7-disubstituerede 3-cephem-4-carboxylsyreforbindelser
US4252951A (en) 1979-10-09 1981-02-24 Eli Lilly And Company Isolation of syn-7-(2-amino-4-thiazolyl)-(methoxyimino)acetamido-3-acetoxymethyl-3-cephem-4-carboxylic acid
JPS58135872A (ja) * 1981-11-13 1983-08-12 グラクソ・グル−プ・リミテツド 新規な化合物およびその製法

Also Published As

Publication number Publication date
GB2119370B (en) 1985-06-05
GB2119370A (en) 1983-11-16
JPS58183678A (ja) 1983-10-26
GR79243B (OSRAM) 1984-10-22
DE3372096D1 (en) 1987-07-23
IL68251A (en) 1986-03-31
DK91383A (da) 1983-10-02
HU186271B (en) 1985-07-29
US4426528A (en) 1984-01-17
EP0091277A2 (en) 1983-10-12
DK91383D0 (da) 1983-02-25
KR840004090A (ko) 1984-10-06
CA1194487A (en) 1985-10-01
EP0091277A3 (en) 1984-12-27
IL68251A0 (en) 1983-06-15

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